Subsurface Transport of Plutonium in Organic and Aqueous Acidic Processing Wastes at the Hanford Site, USA
Not Available
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Engineering topics
Kersting, Annie B.
Publications and source records attributed to Kersting, Annie B..
Radionuclide transport in fractured chalk under abrupt changes in salinity
Internationally, it has been agreed that geologic repositories for spent fuel and radioactive waste are considered the internationally agreed upon solution for intermediate and long-term disposal. In countries where traditional nuclear waste repository host rocks (e.g., clay, salt, granite) are not available, other low permeability lithologies must be studied. Here, chalk is considered to determine its viability for disposal. Despite chalk's low bulk permeability, it may contain fracture networks that can facilitate radionuclide transport. In arid areas, groundwater salinity may change seasonally due to the mixing between brackish groundwater and fresh meteoric water. Such salinity changes may impact the radionuclides' mobility. In this study, radioactive U(VI) and radionuclide simulant tracers (Sr, Ce and Re) were injected into a naturally fractured chalk core. The mobility of tracers was investigated under abrupt salinity variations. Two solutions were used: a low ionic strength (IS) artificial rainwater (ARW; IS ~0.002) and a high IS artificial groundwater (AGW; IS ~0.2). During the experiments, the tracers were added to ARW, then the carrier was changed to AGW, and vice versa. Ce was mobile only in colloidal form, while Re was transported as a conservative tracer. Both Re and Ce demonstrated no change in mobility due to salinity changes. In contrast, U and Sr showed increased mobility when AGW was introduced and decreased mobility when ARW was introduced into the core. These experimental results, supported by reactive transport modeling, suggest that saline groundwater solutions promote U and Sr release via ion-exchange and enhance their migration in fractured chalk. Here the study emphasizes the impact of salinity variations near spent fuel repositories and their possible impact on radionuclide mobility.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Microbial community dynamics and cycling of plutonium and iron in a seasonally stratified and radiologically contaminated pond
Plutonium (Pu) cycling and mobility in the environment can be impacted by the iron cycle and microbial community dynamics. We investigated the spatial and temporal changes of the microbiome in an iron (Fe)-rich, plutonium-contaminated, monomictic reservoir (Pond B, Savannah River Site, South Carolina, USA). The microbial community composition varied with depth during seasonal thermal stratification and was strongly correlated with redox. During stratification, Fe(II) oxidizers (e.g., Ferrovum, Rhodoferax, Chlorobium) were most abundant in the hypoxic/anoxic zones, while Fe(III) reducers (e.g., Geothrix, Geobacter) dominated the deep, anoxic zone. Sulfate reducers and methanogens were present in the anoxic layer, likely contributing to iron and plutonium cycling. Multinomial regression of predicted functions/pathways identified metabolisms highly associated with stratification (within the top 5%), including iron reduction, methanogenesis, C1 compound utilization, fermentation, and aromatic compound degradation. Two sediment cores collected at the Inlet and Outlet of the pond were dominated by putative fermenters and organic matter (OM) degraders. Overall, microbiome analyses revealed the potential for three microbial impacts on the plutonium and iron biogeochemical cycles: (1) plutonium bioaccumulation throughout the water column, (2) Pu–Fe-OM-aggregate formation by Fe(II) oxidizers under microaerophilic/aerobic conditions, and (3) Pu–Fe-OM-aggregate or sediment reductive dissolution and organic matter degradation in the deep, anoxic waters.
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Impact of a Biological Chelator, Lanmodulin, on Minor Actinide Aqueous Speciation and Transport in the Environment
Minor actinides are major contributors to the long-term radiotoxicity of nuclear fuels and other radioactive wastes. Here in this context, understanding their interactions with natural chelators and minerals is key to evaluating their transport behavior in the environment. The lanmodulin family of metalloproteins is produced by ubiquitous bacteria and Methylorubrum extorquens lanmodulin (LanM) was recently identified as one of nature’s most selective chelators for trivalent f-elements. Herein, we investigated the behavior of neptunium, americium, and curium in the presence of LanM, carbonate ions, and common minerals (calcite, montmorillonite, quartz, and kaolinite). We show that LanM’s aqueous complexes with Am(III) and Cm(III) remain stable in carbonate-bicarbonate solutions. Furthermore, the sorption of Am(III) to these minerals is strongly impacted by LanM, while Np(V) sorption is not. With calcite, even a submicromolar concentration of LanM leads to a significant reduction in the Am(III) distribution coefficient (K d , from >10 4 to ~10 2 mL/g at pH 8.5), rendering it even more mobile than Np(V). Thus, LanM-type chelators can potentially increase the mobility of trivalent actinides and lanthanide fission products under environmentally relevant conditions. Monitoring biological chelators, including metalloproteins, and their biogenerators should therefore be considered during the evaluation of radioactive waste repository sites and the risk assessment of contaminated sites.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Sources, seasonal cycling, and fate of plutonium in a seasonally stratified and radiologically contaminated pond
Unlike short-term laboratory experiments, studies at sites historically contaminated with radionuclides can provide insight into contaminant migration behavior at environmentally-relevant decadal timescales. One such site is Pond B, a seasonally stratified reservoir within Savannah River Site (SC, USA) has low levels (μBq L –1 ) of plutonium in the water column. Here, we evaluate the origin of plutonium using high-precision isotope measurements, investigate the impact of water column geochemistry on plutonium cycling during different stratification periods, and re-evaluate long-term mass balance of plutonium in the pond. New isotopic data confirm that reactor-derived plutonium overwhelms input from Northern Hemisphere fallout at this site. Two suggested mechanisms for observed plutonium cycling in the water column include: (1) reductive dissolution of sediment-derived Fe(III)-(oxyhydr)oxides during seasonal stratification and (2) plutonium stabilization complexed strongly to Fe(III)-particulate organic matter (POM) complexes. While plutonium may be mobilized to a limited extent by stratification and reductive dissolution, peak plutonium concentrations are in shallow waters and associated with Fe(III)-POM at the inception of stratification. This suggests that plutonium release from sediments during stratification is not the dominant mechanism driving plutonium cycling in the pond. Importantly, our analysis suggests that the majority is retained in shallow sediments and may become increasingly recalcitrant.
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LLNL SFA OBER FY23 Program Management and Performance Report: BioGeoChemistry at Interfaces
The focus of the BioGeoChemistry at Interfaces SFA has been to identify and quantify the biogeochemical processes and the underlying mechanisms that control actinide mobility in an effort to reliably predict and control the cycling and migration of actinides in the environment. The research approach has included: (1) Field Studies that capture actinide behavior on the timescale of decades (Research Thrust 1), and (2) Fundamental Laboratory Studies that isolate specific biogeochemical processes observed in the field (Research Thrust 2). These Research Thrusts are underpinned by the unique capabilities and staff expertise at Lawrence Livermore National Laboratory, allowing the BioGeoChemistry at Interfaces SFA to advance our understanding of actinide migration behavior in the environment, and serve as a resource for environmental radiochemistry research internationally (Figure 1). In FY23, our SFA research focused on transient redox gradients across stratified waters, sediment-water interfaces, and mineral-water interfaces to address processes controlling cycling of redox-sensitive metals. Nevertheless, Research Thrusts 1 and 2 are guided by the following broad central hypotheses that were developed during our last program review held at the end of FY18: Thrust 1 Hypothesis: Biogeochemical processes occurring on the timescale of years to decades lead to greater actinide recalcitrance in sediments and limits their migration in surface and groundwater. Thrust 2 Hypothesis: Long-term biogeochemical processes include mineral and surface alteration, which leads to stabilization of actinide surface associations or incorporation into mineral precipitates. Our strategic goal is to use the knowledge gained from our Science Plan to advance our understanding of the behavior of actinides and other radionuclides (e.g. Cs) and provide DOE with the scientific basis for remediation and long-term stewardship of DOE’s legacy sites. More broadly, we are improving our understanding of transport phenomena in environmental systems sciences with a particular emphasis on environmentally relevant (long-term) timescales. While we retained some of our historical focus on actinide biogeochemistry this past fiscal year, biogeochemical processes occurring at unique Test Bed locations associated with this SFA provide fundamental information on abiotic and biotic redox processes that control the cycling of redox sensitive metals under dynamic and transient conditions. Furthermore, in collaboration with SFA teams at Argonne National Laboratory, our SFA has begun to transition away from the current research focus and develop a new research program in terrestrial wetland systems. The Terrestrial Wetland Function and Resilience SFA program plan will be delivered to the Environmental System Science (ESS) program within BER at the end of FY23.
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Area V: Waste Management and Subsurface Science (FY23 Q2)
The objective of Topic Area V is to evaluate the feasibility and safety of an intermediate-depth borehole for disposal of IAEC nuclear waste. The IAEC nuclear waste is currently stored in above ground and/or in near-surface facilities that provide short-term radiological worker safety but do not provide long-term, full security and safeguards protection for the nuclear material. Disposal of the IAEC nuclear waste several hundred meters below the surface in a sealed borehole would provide long-term security and safeguards due to its depth underground, as well as long-term radiological safety, due to its isolation in a stable geological formation.
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Temporal evolution of Pu and Cs sediment contamination in a seasonally stratified pond
There remains a lack of knowledge regarding ecosystem transfer, transport processes, and mechanisms, which influence the long-term mobility of Pu-239 and Cs-137 in natural environments. Monitoring the distribution and migration of trace radioisotopes as ecosystem tracers has the potential to provide insight into the underlying mechanisms of geochemical cycles. This study investigated the distribution of anthropogenic radionuclides Pu-239 and Cs-137 along with total organic carbon, iron, and trace element in contaminated sediments of Pond B at the Savannah River Site (SRS). Pond B received reactor cooling water from 1961 to 1964, and trace amounts of Pu-239 and Cs-137 during operations. Our study collected sediment cores to determine concentrations of Pu-239, Cs-137, and major and minor elements in solid phase, pore water and an electrochemical method was used on wet cores to determine dissolved elemental concentrations. More than 50 years after deposition, Pu-239 and Cs-137 in sediments are primarily located in the upper 5 cm in area where deposition of particulate-bound contaminants was prevalent and located between 5 and 10 cm in areas of high sedimentation, showing a limited migration of Pu-239 and Cs-137. A Factor analysis demonstrated different sediment facies across the pond resulting in a range of geochemical processes controlling accumulation of Pu and Cs. Highest concentrations appear to be controlled by particulate input from the influent canal, dominated by clay, silt, and sand minerals bearing Fe. Elevated Pu-239 in the sediments were observed in areas with high organic matter and higher deposition rate relative to the Pond B system near the outlet indicating strong association of Pu with OM and particulates. Therefore, organic matter cycling likely plays a role in Pu redistribution between sediment and overlying pond water, and deposition in organic rich sediments accumulating near the outlet. Though Pu appears to have been distributed throughout the pond, Cs-137 concentrations remained the highest near the influent canal.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Plutonium mobilization from contaminated estuarine sediments, Esk Estuary (UK)
Since 1952, liquid radioactive effluent containing 238-242 Pu, 241 Am, 237 Np, 137 Cs, and 99 Tc has been released with authorization from the Sellafield nuclear complex (UK) into the Irish Sea. This represents the largest source of plutonium (Pu) discharged in all western Europe, with 276 kg having been released. In the Eastern Irish Sea, the majority of the transuranic activity has settled into an area of sediments (Mudpatch) located off the Cumbrian coast. Radionuclides from the Mudpatch have been re-dispersed via particulate transport in fine-grained estuarine and intertidal sediments to the North-East Irish Sea, including the intertidal saltmarsh located at the mouth of the Esk Estuary. Saltmarshes are highly dynamic systems which are vulnerable to external agents (sea level change, erosion, sediment supply, and freshwater inputs), and their stability remains uncertain under current sea level rise projections and possible increases in storm activity. In this work, we examined factors affecting Pu mobility in contaminated sediments collected from the Esk Estuary by conducting leaching experiments under both anoxic and oxic conditions. Here, leaching experiments were conducted over a 9-month period and were periodically sampled to determine solution phase Pu via multicollector-inductively coupled plasma-mass spectrometry (MC-ICP-MS), and to measure redox indicators (Eh, pH and extractable Fe(II)). Microbial community composition was also characterized in the sediments, and at the beginning and end of the anoxic/oxic experiments. Results show that: 1) Pu leaching is about three times greater in solutions leached under anoxic conditions compared to oxic conditions, 2) the sediment slurry microbial communities shift as conditions change from anoxic to oxic, 3) Pu leaching is enhanced in the shallow sediments (0–10 cm depth), and 4) the magnitude of Pu leached from sediments is not correlated with total Pu, indicating that the biogeochemistry of sediment-associated Pu is spatially heterogeneous. These findings provide constraints on the stability of redox sensitive Pu in biogeochemically dynamic/transient environments on a timescale of months and suggests that anoxic conditions can enhance Pu mobility in estuarine systems.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
BioGeoChemistry at Interfaces (LLNL SFA OBER FY22 Program Management and Performance Report)
The focus of the BioGeoChemistry at Interfaces SFA is to identify and quantify the biogeochemical processes and the underlying mechanisms that control actinide mobility in an effort to reliably predict and control the cycling and migration of actinides in the environment. The research approach includes: (1) Field Studies that capture actinide behavior on the timescale of decades (Research Thrust 1), and (2) Fundamental Laboratory Studies that isolate specific biogeochemical processes observed in the field (Research Thrust 2). These Research Thrusts are underpinned by the unique capabilities and staff expertise at Lawrence Livermore National Laboratory, allowing the BioGeoChemistry at Interfaces SFA to advance our understanding of actinide migration behavior in the environment, and serve as an resource for environmental radiochemistry research internationally. In the past year, our greater focus on transient redox gradients across stratified waters, sediment-water interfaces, and mineral-water interfaces extended our research beyond actinides to address processes controlling cycling of redox-sensitive metals more broadly. Nevertheless, Research Thrusts 1 and 2 are guided by the following broad central hypotheses that were developed during our last program review held at the end of FY18: Thrust 1 Hypothesis: Biogeochemical processes occurring on the timescale of years to decades lead to greater actinide recalcitrance in sediments and limits their migration in surface and groundwater. Thrust 2 Hypothesis: Long-term biogeochemical processes include mineral and surface alteration, which leads to stabilization of actinide surface associations or incorporation into mineral precipitates. Our strategic goal is to use the knowledge gained from our Science Plan to advance our understanding of the behavior of actinides and other radionuclides (e.g. Cs) and provide DOE with the scientific basis for remediation and long-term stewardship of DOE’s legacy sites. More broadly, we will enhance our understanding of transport phenomena in environmental systems sciences with a particular emphasis on environmentally relevant (long-term) timescales. While we retain our focus on actinide biogeochemistry, our increased focus on overall biogeochemical processes occurring at unique Test Bed locations associated with this SFA provides fundamental information on abiotic and biotic redox processes that control the cycling of redox sensitive metals under dynamic and transient conditions.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Subsurface microbial communities as a tool for characterizing regional-scale groundwater flow
Subsurface microbial community distribution patterns are influenced by biogeochemical and groundwater fluxes and may inform hydraulic connections along groundwater-flow paths. This study examined the regional-scale microbial community of the Death Valley Regional Flow System and evaluated whether subsurface communities can be used to identify groundwater-flow paths between recharge and discharge areas. Samples were collected from 36 sites in three groundwater basins: Pahute Mesa–Oasis Valley (PMOV), Ash Meadows (AM), and Alkali Flat–Furnace Creek Ranch (AFFCR). Microbial diversity within and between communities varied by location, and communities were separated into two overall groups that affiliated with the AM and PMOV/AFFCR basins. Network analysis revealed patterns between clusters of common microbes that represented groundwaters with similar geochemical conditions and largely corroborated hydraulic connections between recharge and discharge areas. Null model analyses identified deterministic and stochastic ecological processes contributing to microbial community assemblages. Most communities were more different than expected and governed by dispersal limitation, geochemical differences, or undominating processes. However, certain communities from sites located within or near the Nevada National Security Site were more similar than expected and dominated by homogeneous dispersal or selection. Overall, the (dis)similarities between the microbial communities of DVRFS recharge and discharge areas supported previously documented hydraulic connections between: (1) Spring Mountains and Ash Meadows; (2) Frenchman and Yucca Flat and Amargosa Desert; and (3) Amargosa Desert and Death Valley. However, only a portion of the flow path between Pahute Mesa and Oasis Valley could be supported by microbial community analyses, likely due to well-associated artifacts in samples from the two Oasis Valley sites. This study demonstrates the utility of combining microbial data with hydrologic, geologic, and water-chemistry information to comprehensively characterize groundwater systems, highlighting both strengths and limitations of this approach.
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Pu distribution among mixed waste components at the Hanford legacy site, USA and implications to long-term migration
Not Available
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Solubility controls on plutonium and americium release in subsurface environments exposed to acidic processing wastes
To identify the role of waste composition and sediment interactions in controlling Pu and Am mobility in contaminated sediments at Hanford, a legacy nuclear site, Pu and Am concentrations in solutions equilibrated with contaminated sediments from beneath the 216-Z-9 (Z-9) Trench were compared to the solubilities of PuO 2 materials, synthesized by methods representative of the disposed wastes, in the absence of sediments. Furthermore, this work shows that the solubilities of PuO 2 materials synthesized by different methods, and with varying particle sizes, agree with PuO 2 (am,hyd), although dissolution kinetics differed between materials. According to saturation index (SI) calculations, PuO 2 (am,hyd) is likely also controlling Pu release from sediments under conditions where phosphate concentrations are low. However, both Pu-phosphate and Am-phosphate phases, identified in SI calculations and by high resolution transmission electron microscopy, play roles in controlling release in low pH, high phosphate, shallow sediments just below the Z-9 Trench. The elevated phosphate is likely due to decomposition of tributyl phosphate from waste solutions over time. Sediments from deeper in the subsurface beneath the Z-9 Trench are less acidic and contain less phosphate, with Pu solubility likely controlled by PuO 2 (am,hyd) that precipitated following neutralization of the acidic waste stream. Controls on Am concentrations in deeper sediments are more complex and potentially involve sediment adsorption and/or release from Pu (1-x) Am x O 2 following Am in-growth. The concentrations of both Pu and Am were elevated in the colloidal fraction associated with shallow sediments, but not in PuO 2 experiments, suggesting the presence of Pu/Am pseudocolloids (e.g., Pu/Am associated with mineral colloids). However, Pu and Am association with the colloidal size fraction was not observed in deeper sediments, suggesting transport of Pu and Am to these depths beneath the Z-9 Trench was not due to colloidal transport.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Plutonium Co-precipitation with Calcite
The mobility of plutonium (Pu) in the environment is affected by Pu–mineral interactions, such as adsorption–desorption and structural incorporation. Calcite (CaCO 3 ) is a common secondary phase in near surface environments and a major component of many rocks and soils and is expected to form as an alteration product of cement-based materials planned for use in geological repositories. The reactivity of the calcite surface and its ability to tolerate significant variations in its chemical composition through substitution of Ca for other cations make calcite a potentially important sink for environmental contaminants. Here, single crystals of calcite were synthesized from aqueous solutions in equilibrium with air containing Pu as either Pu(VI) or Pu(IV) and characterized using a combination of laser ablation inductively coupled plasma mass spectrometry (LA–ICP–MS) and X-ray absorption spectroscopy (XAS). These data are used to assess the amount, structure, and oxidation state of Pu co-precipitated into calcite, providing insight into the potential for Pu sequestration in calcite precipitates. Overall, the XAS and LA–ICP–MS data support the co-precipitation of plutonyl [Pu(VI/V)] in the bulk calcite, although the exact nature of the co-precipitated Pu complex is difficult to elucidate in the synthesized material. Co-precipitated plutonyl could be incorporated in either distorted Ca lattice sites or defect sites, and we provide evidence to suggest that Pu(VI) is reduced mainly to Pu(V) in the precipitated solid. LA–ICP–MS additionally shows that the co-precipitation of Pu(VI/V) is favored over the co-precipitation of Pu(IV). Altogether, our results suggest that Pu sequestration in calcite under environmental conditions could immobilize Pu and isolate it from groundwater interactions in contaminated environments.
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Characterization of Americium and Curium Complexes with the Protein Lanmodulin: A Potential Macromolecular Mechanism for Actinide Mobility in the Environment
Anthropogenic radionuclides, including long-lived heavy actinides such as americium and curium, represent the primary long-term challenge for management of nuclear waste. The potential release of these wastes into the environment necessitates understanding their interactions with biogeochemical compounds present in nature. Here, we characterize the interactions between the heavy actinides, Am 3+ and Cm 3+ , and the natural lanthanide-binding protein, lanmodulin (LanM). LanM is produced abundantly by methylotrophic bacteria, including Methylorubrum extorquens, that are widespread in the environment. We determine the first stability constant for an Am 3+ -protein complex (Am 3 LanM) and confirm the results with Cm 3 LanM, indicating a ~5-fold higher affinity than that for lanthanides with most similar ionic radius, Nd 3+ and Sm 3+ , and making LanM the strongest known heavy actinide-binding protein. The protein’s high selectivity over 243 Am’s daughter nuclide 239 Np enables lab-scale actinide-actinide separations as well as provides insight into potential protein-driven mobilization for these actinides in the environment. The luminescence properties of the Cm 3+ -LanM complex, and NMR studies of Gd 3+ -LanM, reveal that lanmodulin-bound f-elements possess two coordinated solvent molecules across a range of metal ionic radii. Finally, we show under a wide range of environmentally relevant conditions that lanmodulin effectively outcompetes desferrioxamine B, a hydroxamate siderophore previously proposed to be important in trivalent actinide mobility. Overall, these results suggest that natural lanthanide-binding proteins such as lanmodulin may play important roles in speciation and mobility of actinides in the environment; it also suggests that protein-based biotechnologies may provide a new frontier in actinide remediation, detection, and separations.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
BioGeoChemistry at Interfaces (LLNL SFA OBER FY21 Program Management and Performance Report)
The focus of the BioGeoChemistry at Interfaces (formerly BioGeoChemistry of Actinides) SFA is to identify and quantify the biogeochemical processes and the underlying mechanisms that control actinide mobility in an effort to reliably predict and control the cycling and migration of actinides in the environment. The research approach includes: (1) Field Studies (Research Thrust 1) that capture actinide behavior on the timescale of decades and (2) Fundamental Laboratory Studies (Research Thrust 2) that isolate specific biogeochemical processes observed in the field. These Research Thrusts are underpinned by the unique capabilities and staff expertise at Lawrence Livermore National Laboratory, allowing the BioGeoChemistry at Interfaces SFA to advance our understanding of actinide migration behavior in the environment, and serve as an international resource for environmental radiochemistry research (Figure 1).
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
The coordination properties and ionic radius of actinium: A 120-year-old enigma
Actinium is an elusive element with untamed properties and represents a peculiar case in the periodic table, as its isotopes are all radioactive, the longest-lived one having only a 22-year half-life, and the availability of actinium isotopes remains very low (microgram level, at best), hindering research on its compounds. Despite being a natural element discovered more than 120 years ago, and despite an increasing interest in using one of its isotopes ( 225 Ac) for highly efficient cancer therapies, the chemistry of actinium is still largely unknown relative to other elements. Since Ac is the first element of the actinide series, it is accepted that its ion, Ac 3+ , is the most voluminous trivalent cation of the periodic table. However, the structural data available on Ac 3+ compounds are scarce and have mainly been collected in the 1940-1960's, when actinide chemistry was still in its infancy, and have not been put in perspective with the advances in the chemistry of other elements, making it difficult to accurately evaluate its actual size and coordination chemistry. Here, we review progress made on the chemistry of lanthanides and actinides and reevaluate the structural data published on Ac 3+ since the era of the Manhattan Project. The data are combined across different spectroscopic and characterization methods and presented in the context of periodic trends. When considering crystallographic data, solution chemistry results, and the nuclear properties of actinium isotopes, it appears that some structural parameters ascribed to the Ac 3+ ion may have been overestimated. This review can guide researchers interested in actinide sciences and those who are pursuing the development of actinium-based radiotherapies, from isotope production to clinical trials.
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